In 1898, at the age of 23, he was selected due to his education to be trained in the United States as a missionary. On July 10, 1898, Aggrey agreed and left the Gold Coast for the United States, where he settled in Salisbury, North Carolina, and attended the Livingstone College. He studied a variety of subjects at the university, including chemistry, physics, logic, economics and politics. In May 1902 he graduated from the university with three academic degrees. Aggrey was very talented in language and was said to have spoken (beside English) French, German, Ancient and Modern Greek, and Latin.
In November 1903 he was appointed the minister of the African Methodists Zion church in Salisbury. In 1905 he married Rose Douglas, a native of Virginia, with whom he had four children. In the same year he began to teach at Livingstone College. In 1912 he earned his doctorate in theology, and in 1914 followed a doctorate in osteopathy. In the same year he transferred employment to a small municipality to North Carolina. Between 1915 and 1917 Aggrey took up further studies at what is now known as Columbia University, where he studied sociology, psychology and the Japanese language.
In 1920 Paul Monroe, a member of the Phelps Stokes Fund offered Aggrey the opportunity to attend a research expedition to Africa to determine which measures were necessary for the improvement of education in Africa. Aggrey accepted and visited what are now ten different countries in Africa, where he collected and analyzed education data. In 1920 he visited Sierra Leone, Liberia, the Gold Coast, Cameroon and Nigeria. In 1921 he visited the Belgian Congo, Angola and South Africa.
During this journey Aggrey made a significant impression and underscored the importance of education among some people who would become important figures in Africa, including Hastings Kamuzu Banda, later president of Malawi, Nnamdi Azikiwe, the first president of Nigeria, and Kwame Nkrumah, the first president of Ghana.
In Ghana he delivered a lecture that persuaded Governor Guggisberg that Achimota College should be co-educational:He was the first vice Principal of Achimota College.
“The surest way to keep people down is to educate the men and neglect the women. If you educate a man you simply educate an individual, but if you educate a woman, you educate a whole nation"